4.8 Article

Multifunctional Catalyst CuS for Nonaqueous Rechargeable Lithium-Oxygen Batteries

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 42, Pages 50065-50075

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c16231

Keywords

lithium-oxygen battery; cathode catalyst; redox mediator; density functional theory; copper sulfide

Funding

  1. National Natural Science Foundation of China [21776176]

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By experiment and theoretical calculation, the different catalytic performance and abnormal discharge plateau phenomenon of two morphologies of copper sulfide in lithium-oxygen batteries were investigated.
Copper sulfide with flower-like (CuS) and carambola-like (c-CuS) morphologies was successfully synthesized by a facile one-step solvothermal route with different surfactants. When employed as cathode catalysts for lithium-oxygen batteries (LOBs), f-CuS outperforms c-CuS in terms of oxygen electrochemistry, judging from the faster kinetics and the higher reversibility of oxygen reduction/oxidation reactions, as well as the better LOB performance. Moreover, an abnormal high-potential discharge plateau was observed in the discharge profile of the LOB. To understand the different performances of f-CuS and c-CuS and the abnormal high-potential plateau, theoretical calculations were conducted, based on which a mechanism was proposed and verified with experiments. On the whole, CuS can work as a multifunctional catalyst for promoting LOB performance, which means that the dissolved CuS in LiTFSI/TEGDME electrolyte can serve as a liquid catalyst by the redox couples of Cu(TFSI)(2)/Cu(TFSI)(2)(-)/Cu(TFSI)(2)(2)(-), in addition to the function as a traditional solid catalyst in the cathode.

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